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Radiative cooling forms an emerging direction in which objects are passively cooled via thermal radiation to cold space. Cooling materials should provide high thermal emissivity (infrared absorptance) and low solar absorptance, making cellulose an ideal and sustainable candidate. Broadband solar-reflective or transparent coolers are not the only systems of interest, but also more pleasingly looking colored systems. However, solutions based on wavelength-selective absorption generate not only color but also heat and thereby counteract the cooling function. Intended as coatings for solar cells, we demonstrate a transreflective cellulose material with minimal solar absorption that generates color by wavelength-selective reflection, while it transmits other parts of the solar spectrum. Our solution takes advantage of the ability of cellulose nanocrystals to self-assemble into helical periodic structures, providing nonabsorptive films with structurally colored reflection. Application of violet-blue, green, and red cellulose films on silicon substrates reduced the temperature by up to 9 degrees C under solar illumination, as result of a combination of radiative cooling and reduced solar absorption due to the wavelength-selective reflection by the colored coating. The present work establishes self-assembled cellulose nanocrystal photonic films as a scalable photonic platform for colored radiative cooling. Funding Agencies|Knut and Alice Wallenberg foundation; Linkoping University; Wallenberg Wood Science Center; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University [2009 00971]; Swedish Foundation for Strategic Research; Wenner-Gren Foundations; Olle Engkvist Foundation [194-0679]; Swedish Research Council

Reconfigurable devices offer the ability to program electronic circuits on demand. In this work, we demonstrated on-demand creation of artificial neurons, synapses, and memory capacitors in post-fabricated perovskite NdNiO3devices that can be simply reconfigured for a specific purpose by single-shot electric pulses. The sensitivity of electronic properties of perovskite nickelates to the local distribution of hydrogen ions enabled these results. With experimental data from our memory capacitors, simulation results of a reservoir computing framework showed excellent performance for tasks such as digit recognition and classification of electrocardiogram heartbeat activity. Using our reconfigurable artificial neurons and synapses, simulated dynamic networks outperformed static networks for incremental learning scenarios. The ability to fashion the building blocks of brain-inspired computers on demand opens up new directions in adaptive networks.

Radiative cooling passively removes heat from objects via emission of thermal radiation to cold space. Suitable radiative cooling materials absorb infrared light while they avoid solar heating by either reflecting or transmitting solar radiation, depending on the application. Here, we demonstrate a reflective radiative cooler and a transparent radiative cooler solely based on cellulose derivatives manufactured via electrospinning and casting, respectively. By modifying the microstructure of cellulose materials, we control the solar light interaction from highly reflective (> 90%, porous structure) to highly transparent (approximate to 90%, homogenous structure). Both cellulose materials show high thermal emissivity and minimal solar absorption, making them suitable for daytime radiative cooling. Used as coatings on silicon samples exposed to sun light at daytime, the reflective and transparent cellulose coolers could passively reduce sample temperatures by up to 15 degrees C and 5 degrees C, respectively. Funding Agencies|Linkoping University

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 ...

Radiative cooling passively removes heat from objects via emission of thermal radiation to cold space. Suitable radiative cooling materials absorb infrared light while they avoid solar heating by either reflecting or transmitting solar radiation, depending on the application. Here, we demonstrate a reflective radiative cooler and a transparent radiative cooler solely based on cellulose derivatives manufactured via electrospinning and casting, respectively. By modifying the microstructure of cellulose materials, we can control the solar light interaction from highly reflective (>90%, porous structure) to highly transparent (≈90%, homogenous structure). Both cellulose materials show strong thermal emissivity and minimal solar absorption, making them suitable for daytime radiative cooling. Used as coatings on silicon samples exposed to sun light at daytime, the reflective and transparent cellulose coolers could passively reduce sample temperatures by up to 32 °C and 15 °C, respectively.

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.

Certain bird species have evolved spectacular colors that arise from organized nanostructures of melanin. Its high refractive index (similar to 1.8) and broadband absorptive properties enable vivid structural colors that are nonsusceptible to photo-bleaching. Mimicking natural melanin structural coloration could enable several important applications, in particular, for non-iridescent systems with colors that are independent of incidence angle. Here, we address this by forming melanin photonic crystal microdomes by inkjet printing. Owing to their curved nature, the microdomes exhibit noniridescent vivid structural coloration, tunable throughout the visible range via the size of the nanoparticles. Large-area arrays (>1 cm(2)) of high-quality photonic microdomes could be printed on both rigid and flexible substrates. Combined with scalable fabrication and the nontoxicity of melanin, the presented photonic microdomes with noniridescent structural coloration may find use in a variety of applications, including sensing, displays, and anticounterfeit holograms. Funding Agencies|Wenner-Gren Foundation; Swedish Research CouncilSwedish Research Council; Knut and Alice Wallenberg foundationKnut & Alice Wallenberg Foundation; Swedish Foundation for Strategic researchSwedish Foundation for Strategic Research; Linkoping University; Wallenberg Wood Science Center the Wallenberg Wood Science Centre; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]

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

Precise manipulation of light-matter interactions has enabled a wide variety of approaches to create bright and vivid structural colors. Techniques utilizing photonic crystals, Fabry-Perot cavities, plasmonics, or high-refractive-index dielectric metasurfaces have been studied for applications ranging from optical coatings to reflective displays. However, complicated fabrication procedures for sub-wavelength nanostructures, limited active areas, and inherent absence of tunability of these approaches impede their further development toward flexible, large-scale, and switchable devices compatible with facile and cost-effective production. Here, a novel method is presented to generate structural color images based on monochromic conducting polymer films prepared on metallic surfaces via vapor phase polymerization and ultraviolet (UV) light patterning. Varying the UV dose enables synergistic control of both nanoscale film thickness and polymer permittivity, which generates controllable structural colors from violet to red. Together with grayscale photomasks this enables facile fabrication of high-resolution structural color images. Dynamic tuning of colored surfaces and images via electrochemical modulation of the polymer redox state is further demonstrated. The simple structure, facile fabrication, wide color gamut, and dynamic color tuning make this concept competitive for applications like multifunctional displays. Funding Agencies|Swedish Foundation for Strategic Research (SSF)Swedish Foundation for Strategic Research; Knut and Alice Wallenberg FoundationKnut & Alice Wallenberg Foundation; Swedish Research Council (VR)Swedish Research Council; Wenner-Gren Foundations; Swedish Government Strategic Research Area in Materials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]

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.

Muscovite type mica is an inorganic material most commonly used in various electronic devices. We use the near-field imaging and nano-FTIR techniques to investigate the properties of mica exfoliated on different substrates. In order to support experimental results, we use a theoretical model and simulation.

Enveloped viruses, such as HIV, Ebola and Influenza, are among the most deadly known viruses. Cellular membrane penetration of enveloped viruses is a critical step in the cascade of events that lead to entry into the host cell. Conventional ensemble fusion assays rely on collective responses to membrane fusion events, and do not allow direct and quantitative studies of the subtle and intricate fusion details. Such details are accessible via single particle investigation techniques, however. Here, we implement nano-infrared spectroscopic imaging to investigate the chemical and structural modifications that occur prior to membrane fusion in the single archetypal enveloped virus, influenza X31. We traced in real-space structural and spectroscopic alterations that occur during environmental pH variations in single virus particles. In addition, using nanospectroscopic imaging we quantified the effectiveness of an antiviral compound in stopping viral membrane disruption (a novel mechanism for inhibiting viral entry into cells) during environmental pH variations.

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 thermal stability of InN layers grown on sapphire by high-pressure chemical vapor deposition has been studied by thermal desorption, atomic force microscopy, X-ray diffraction, and infrared reflection measurements. Desorption products from samples grown with group V/III precursor ratios from 1200 to 4800, but otherwise identical growth conditions, have been monitored using differentially-pumped mass spectrometry while the sample temperature was ramped from room temperature to 825 °C. No significant desorption of nitrogen from the surface was observed below 630 °C, with a rapid increase of desorption of molecular nitrogen at substrate temperatures above 630 °C. No significant desorption of NH*/NH2* fragments was observed. From Arrhenius plots, the activation energy for desorption of nitrogen was found to be 1.6 ± 0.2 eV. It was observed that the activation energy for the desorption of nitrogen from InN samples was independent of V/III precursor ratio. However, the temperature corresponding to the maximum desorption was found to be dependent on V/III precursor ratio, increasing from 749 °C for V/III precursor ratio of 1200 to 776 °C for V/III precursor ratio of 4800. The observed shift in the peak desorption temperature with increasing group V/III precursor ratio is attributed to the decrease in extended defects and the increase in grain size.

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.

This contribution presents results on achievable growth temperatures and growth rates as a function of reactor pressure for the growth of InN by high-pressure chemical vapour deposition (HPCVD). The InN epilayers were grown at reactor pressures ranging from atmospheric pressure to 19 bar. The results show that the InN growth temperature increased linearly with the reactor pressure from 759 °C to 876 °C. The growth rate decreases from 127 nm/h to 20 nm/h as the reactor pressure is increased from 1 bar to 19 bar. The structural, optical, and electrical properties of the epitaxial layers were analyzed by X-ray diffraction, Raman spectroscopy, IR reflection spectroscopy, and optical transmission spectroscopy. (© 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

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.

The influences of reactor pressure on the stoichiometry, free carrier concentration, IR and Hall determined mobility, effective optical band edge, and optical phonon modes of HPCVD grown InN films have been analysed and are reported. The In 3d, and N 1s XPS spectra results revealed In-N and N-In bonding states as well as small concentrations of In-O and N-O bonds, respectively in all samples. InN layers grown at 1 bar were found to contain metallic indium, suggesting that the incorporation of nitrogen into the InN crystal structure was not efficient. The free carrier concentrations, as determined by Hall measurements, were found to decrease with increasing reactor pressure from 1.61×1021 to 8.87×1019 cm-3 and the room-temperature Hall mobility increased with reactor pressure from 21.01 to 155.18 cm2/Vs at 1 and 15 bar reactor pressures, respectively. IR reflectance spectra of all three (1, 8, and 15 bar) InN samples were modelled assuming two distinct layers of InN, having different free carrier concentration, IR mobility, and effective dielectric function values, related to a nucleation/interfacial region at the InN/sapphire, followed by a bulk InN layer. The effective optical band gap has been found to decrease from 1.19 to 0.95 eV with increasing reactor pressure. Improvement of the local structural quality with increasing reactor pressure has been further confirmed by Raman spectroscopy measurements. (© 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)

The influence of structural and optoelectronic properties of InN epilayers on the duration of initial nucleation has been studied. High pressure chemical vapor deposition (HPCVD) has been utilized to deposit InN epilayers on GaN/sapphire (0001) templates at a reactor pressure of 15 bar. The initial nucleation period was varied between 10 s and 60 s, leaving all other growth parameters constant. The structural properties of the grown samples have been investigated by X-ray diffraction (XRD) spectroscopy and Raman spectroscopy. The optoelectronic properties were analyzed by Fourier transform infra-red (FTIR) spectroscopy. The layer thickness, free carrier concentration and void fraction were obtained by simulating IR spectra, using multi-layer stack model for epilayers and Lorentz-Drude model for dielectric function. Raman, X-ray diffraction (XRD) and void fraction calculation results suggest that the optimum nucleation time is between 10 - 20 s. However, simulation results revealed that the free carrier concentration of the bulk layer does not show any significant dependency on the duration of initial nucleation.

The dependency of the structural and optoelectronic properties of InN thin films grown by high-pressure chemical vapor deposition technique on the group V/III molar precursor ratio has been studied. X-ray diffraction, Raman spectroscopy, and IR reflectance spectroscopy have been utilized to study local- and long-range structural ordering as well as optoelectronic properties of the InN epilayers grown on crystalline sapphire substrates. The investigated InN epilayers were grown with group V/III molar precursor ratio varying from 900 to 3600, while all other growth parameters were kept constant. For a group V/III precursor ratio of 2400, the full width-half maximum of the Raman E2(high) mode and XRD (0002) Bragg reflex exhibit minimums of 7.53 cm⁻¹ and 210 arcsec, respectively, with maximized grain size and reduced in-plane strain effect. FTIR data analysis revealed a growth rate of 120 nm/hr, a carrier mobility of 1020 cm²V⁻¹s⁻¹, and a free carrier concentration of 1.7×10 18 cm⁻³ for a V/III ratio of 2400. The Raman analysis indicate that non-polar E2(high) mode remains unaffected from a changing V/III ratio; whereas, polar A1(LO) mode significantly changes with changing V/III ratio. Optical analysis also suggests that LO-phonon correlates with free carrier concentration (ne) and TO-phonon correlates with free carrier mobility (µ) in the InN epilayers.

Results on the achievable growth temperature as a function of the reactor pressure for the growth of InN by high-pressure CVD are presented. As the reactor pressure was increased from 1 bar to 19 bar, the optimal growth temperature raised from 759°C to 876°C, an increase of 6.6 °C/bar. The InN layers were grown in a horizontal flow channel reactor, using a pulsed precursor injection scheme. The structural and optical properties of the epilayers have been investigated by Raman spectroscopy, X-ray diffraction, and IR reflectance spectroscopy.

The influence of the growth temperature on the phase stability and composition of single-phase In1-xGaxN epilayers has been studied. The In1-xGaxN epilayers were grown by high-pressure Chemical Vapor Deposition with nominally composition of x = 0.6 at a reactor pressure of 15 bar at various growth temperatures. The layers were analyzed by x-ray diffraction, optical transmission spectroscopy, atomic force microscopy, and Raman spectroscopy. The results showed that a growth temperature of 925°C led to the best single phase InGaN layers with the smoothest surface and smallest grain areas

The influence of super-atmospheric reactor pressures (2.5‐18.5bar) on the electrical and structural properties of InN epilayers deposited on GaN/sapphire (0001) templates by high-pressure chemical vapor deposition has been studied. The epilayers were analyzed by Raman, x-ray diffraction (XRD), and Fourier transform infrared reflectance spectrometry to determine the structural properties as well as the phonon frequencies, dielectric function, plasma frequency, layer thickness and damping parameters of the epilayers. For the studied process parameter space, best material properties were achieved at a reactor pressure of 12.5bar and a group-V/III ratio of 2500 with a free carrier concentration of 1.5 � 10 18 cm � 3 , a mobility of the bulk InN layer of 270 cm 2 V � 1 s � 1 , and a Raman (E2 high) FWHM value of 10.3cm � 1 . This study shows that the crystalline layer properties—probed by XRD 2h‐x scans—improve with increasing reactor pressure. V C 2012