Using localized surface plasmon resonances (LSPR) to focus electromagnetic radiation to the nanoscale shows the promise of unprecedented capabilities in optoelectronic devices, medical treatments and nanoscale chemistry, due to a strong enhancement of light-matter interactions. As we continue to explore novel applications, we require a systematic quantitative method to compare suitability across different geometries and a growing library of materials. In this work, we propose application-specific figures of merit constructed from fundamental electronic and optical properties of each material. We compare 17 materials from four material classes (noble metals, refractory metals, transition metal nitrides, and conductive oxides) considering eight topical LSPR applications. Our figures of merit go beyond purely electromagnetic effects and account for the materials’ thermal properties, interactions with adjacent materials, and realistic illumination conditions. For each application we compare, for simplicity, an optimized spherical antenna geometry and benchmark our proposed choice against the state-of-the-art from the literature. Our propositions suggest the most suitable plasmonic materials for key technology applications and can act as a starting point for those working directly on the design, fabrication, and testing of such devices.
This perspective considers the enormous promise of epitaxial functional transition metal oxide thin films for future applications in low power electronic and energy applications since they offer wide-ranging and highly tunable functionalities and multifunctionalities, unrivaled among other classes of materials. It also considers the great challenges that must be overcome for transition metal oxide thin films to meet what is needed in the application domain. These challenges arise from the presence of intrinsic defects and strain effects, which lead to extrinsic defects. Current conventional thin film deposition routes often cannot deliver the required perfection and performance. Since there is a strong link between the physical properties, defects and strain, routes to achieving more perfect materials need to be studied. Several emerging methods and modifications of current methods are presented and discussed. The reasons these methods better address the perfection challenge are considered and evaluated.
Materials such as W, TiN, and SrRuO (SRO) have been suggested as promising alternatives to Au and Ag in plasmonic applications owing to their stability at high operational temperatures. However, investigation of the reproducibility of the optical properties after thermal cycling between room and elevated temperatures is so far lacking. Here, thin films of W, Mo, Ti, TiN, TiON, Ag, Au, SrRuO and SrNbO are investigated to assess their viability for robust refractory plasmonic applications. These results are further compared to the performance of SrMoO reported in literature. Films ranging in thickness from 50 to 105 nm are deposited on MgO, SrTiO and Si substrates by e-beam evaporation, RF magnetron sputtering and pulsed laser deposition, prior to characterisation by means of AFM, XRD, spectroscopic ellipsometry, and DC resistivity. Measurements are conducted before and after annealing in air at temperatures ranging from 300 to 1000° C for one hour, to establish the maximum cycling temperature and potential longevity at elevated temperatures for each material. It is found that SrRuO retains metallic behaviour after annealing at 800° C, while SrNbO undergoes a phase transition resulting in a loss of metallic behaviour after annealing at 400° C. Importantly, the optical properties of TiN and TiON are degraded as a result of oxidation and show a loss of metallic behaviour after annealing at 500° C, while the same is not observed in Au until annealing at 600° C. Nevertheless, both TiN and TiON may be better suited than Au or SRO for high temperature applications operating under vacuum conditions.
Strontium molybdate (SrMoO3) thin films are grown epitaxially on strontium titanate (SrTiO3), magnesium oxide (MgO), and lanthanum aluminate (LaAlO3) substrates by pulsed laser deposition and possess electrical resistivity as low as 100 µΩ cm at room temperature. SrMoO3 is shown to have optical losses, characterized by the product of the Drude broadening, ΓD, and the square of the plasma frequency, ωpu2, significantly lower than TiN, though generally higher than Au. Also, it is demonstrated that there is a zero‐crossover wavelength of the real part of the dielectric permittivity, which is between 600 and 950 nm (2.05 and 1.31 eV), as measured by spectroscopic ellipsometry. Moreover, the epsilon near zero (ENZ) wavelength can be controlled by engineering the residual strain in the films, which arises from a strain dependence of the charge carrier concentration, as confirmed by density of states calculations. The relatively broad tunability of ENZ behavior observed in SrMoO3 demonstrates its potential suitability for transformation optics along with plasmonic applications in the visible to near infrared spectral range.
In the search for alternative plasmonic materials SrMoO3 has recently been identified as possessing a number of desirable optical properties. Owing to the requirement for many plasmonic devices to operate at elevated temperatures however, it is essential to characterize the degradation of these properties upon heating. Here, SrMoO3 thin films are annealed in air at temperatures ranging from 75 -500° C. Characterizations by AFM, XRD, and spectroscopic ellipsometry after each anneal identify a loss of metallic behaviour after annealing at 500° C, together with the underlying mechanism. Moreover, it is shown that by annealing the films in nitrogen following deposition, an additional crystalline phase of SrMoO4 is induced at the film surface, which suppresses oxidation at elevated temperatures. ExperimentalThe SrMoO3 PLD target material was prepared from SrMoO4 powder (99.9% purity) supplied by Alfa Aesar. The powder was placed in propan-2-ol and ball milled at 300 rpm for 20 hrs before evaporating the propan-2-ol by placing the powder in an oven overnight at 60° C. The powder was then reduced in a furnace under 100 mL min -1 gas flow of 5% H2 / 95% N2 at 1400° C for 10 hrs. The powder was then pressed into a target with a density of approximately 4 g cm -3 before sintering under the same gas flow conditions at 1500° C for 12 hours.The SrMoO3 target material was rotated throughout each pulsed laser deposition process and held 60 mm from the SrTiO3 substrate. A KrF excimer laser (240 nm) was used for the deposition of all samples with a repetition rate of 8 Hz and a 10 s relaxation period after every 20 pulses. A laser fluency of 1.2 J cm -2 was used. Vacuum conditions, approximately 1×10 -7 Torr, were used for the deposition of all samples and the substrate temperature was 650° C. The samples were cooled to room temperature after each deposition process at a rate of 10° C min -1 , either in vacuum or following annealing in 500 Torr N2 (6N purity, supplied by BOC), prior to removal from the vacuum chamber. Single side polished 5x5 mm (100) oriented STO substrates with a thickness of 0.5 mm were used.An IONTOF ToF-SIMS 5 instrument was used for SIMS depth profiling of the samples. An area of 100x100 μm 2 was analysed using a 25 keV Bi+ LMIG in high current bunch mode with a beam current of approximately 1 pA. Only negative secondary ions were collected. For depth profiling, a 1 keV Cs+ ion beam with a current of 75 nA was used, giving a sputter crater area of 300x300 μm 2 .The surfaces of the SMO films before and after annealing were characterised using X-ray photoelectron spectroscopy (XPS). The spectra were recorded on a Thermo Scientific K-Alpha+ spectrometer operating at a base pressure of 2x10 -9 mbar. This system incorporates a monochromated, microfocused Al Kα X-ray source (hν = 1486.6 eV) and a 180° double focusing hemispherical analyser with a 2D detector. The X-ray source was operated a 6 mA emission current and 12 kV anode bias. Data were collected at pass energies of 200 eV for survey, and 20 eV for core le...
First time demonstration of epitaxially stabilised δ-Bi2O3 phase in vertically aligned nanocomposite thin films, exhibiting very high ionic conductivities of up to 10−3 S cm−1 at 500 °C.
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