Titanium nitride (TiN) is an interesting refractory metallic compound which could replace gold as an alternative plasmonic material, especially for high temperature and semiconductor compatible applications. However, reported plasmonic properties of TiN films are so far limited by conventional growth techniques, such as reactive sputtering. In this work, we adopt the nitrogen-plasma-assisted molecular-beam epitaxy (MBE) to grow single-crystalline, stoichiometric TiN films on sapphire substrates. The properties of as-grown TiN epitaxial films have been fully characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), spectroscopic ellipsometry (SE), and surface plasmon polariton (SPP) interferometry. We have confirmed that MBE-grown TiN films exhibit excellent plasmonic properties to replace gold in the visible and near-infrared spectral regions. Measuring the real and imaginary parts of dielectric function by SE, it is also found that TiN is better than gold in the shortwavelength range (<500 nm), where gold suffers from strong loss due to interband transition. Contrary to the recent theoretical prediction that air is not able to stabilize SPP modes at the TiN surface, our surface plasmon interferometry data clearly show the presence of propagating SPP modes at the TiN/air interface. To demonstrate the unique plasmonic properties of MBEgrown stoichiometric TiN, we have fabricated TiN metasurfaces for the visible-spectrum applications.

In comparison to noble metals (gold and silver), aluminum is a sustainable and widely applicable plasmonic material owing to its abundance in the Earth’s crust and compatibility with the complementary metal–oxide–semiconductor (CMOS) technology for integrated devices. Aluminum (Al) has a superior performance in the ultraviolet (UV) regime with the lowest material loss and good performance in the full visible regime. Furthermore, aluminum films can remain very stable in ambient environment due to the formation of surface native oxide (alumina) acting as a passivation layer. In this work, we develop an epitaxial growth technique for forming atomically smooth aluminum films on transparent c-plane (0001) sapphire (Al-on-Sapphire, ALOSA) by molecular-beam epitaxy (MBE). The MBE-grown ALOSA films have small plasmonic losses and enable us to fabricate and utilize high-quality plasmonic nanostructures in a variety of optical configurations (reflection, transmission, and scattering). Here, the surface roughness and crystal orientation of ALOSA films are characterized by atomic force microscopy (AFM) and X-ray diffraction (XRD). Moreover, the formation of smooth native oxide layer and abrupt heterointerfaces are investigated by transmission electron microscopy (TEM). We have also measured the optical dielectric function of epitaxial aluminum films by using spectroscopic ellipsometry (SE). These results show that the structural and optical properties of epitaxial aluminum films grown by MBE are excellent compared to polycrystalline aluminum films grown by other deposition methods. To illustrate the capability of device applications for the full visible spectrum, we demonstrate clear surface plasmon polarition (SPP) interference patterns using a series of double-groove surface interferometer structures with varied groove–groove separations under white-light illumination. Finally, we show the device performance of zinc oxide (ZnO) nanowire (UV) and indium gallium nitride (InGaN) nanorod (blue and green) plasmonic lasers prepared by using the epitaxial Al films. The measured lasing thresholds are comparable with the best available data obtained on the Ag films. According to these result, we suggest that epitaxial ALOSA films are a versatile plasmonic material platform in the UV and full visible spectral regions.

Plasmonics have been well investigated on photodetectors, particularly in IR and visible regimes. However, for a wide range of ultraviolet (UV) applications, plasmonics remain unavailable mainly because of the constrained optical properties of applicable plasmonic materials in the UV regime. Therefore, an epitaxial single-crystalline aluminum (Al) film, an abundant metal with high plasma frequency and low intrinsic loss is fabricated, on a wide bandgap semiconductive gallium nitride (GaN) to form a UV photodetector. By deliberately designing a periodic nanohole array in this Al film, localized surface plasmon resonance and extraordinary transmission are enabled; hence, the maximum responsivity (670 A W −1) and highest detectivity (1.48 × 10 15 cm Hz 1/2 W −1) is obtained at the resonance wavelength of 355 nm. In addition, owing to coupling among nanoholes, the bandwidth expands substantially, encompassing the entire UV range. Finally, a Schottky contact is formed between the single-crystalline Al nanohole array and the GaN substrate, resulting in a fast temporal response with a rise time of 51 ms and a fall time of 197 ms. To the best knowledge, the presented detectivity is the highest compared with those of other reported GaN photodetectors.

Graphene is a two-dimensional (2D) structure that creates a linear relationship between energy and momentum that not only forms massless Dirac fermions with extremely high group velocity but also exhibits a broadband transmission from 300 to 2500 nm that can be applied to many optoelectronic applications, such as solar cells, light-emitting devices, touchscreens, ultrafast photodetectors, and lasers. Although the plasmonic resonance of graphene occurs in the terahertz band, graphene can be combined with a noble metal to provide a versatile platform for supporting surface plasmon waves. In this study, we propose a hybrid graphene–insulator–metal (GIM) structure that can modulate the surface plasmon polariton (SPP) dispersion characteristics and thus influence the performance of plasmonic nanolasers. Compared with values obtained when graphene is not used on an Al template, the propagation length of SPP waves can be increased 2-fold, and the threshold of nanolasers is reduced by 50% when graphene is incorporated on the template. The GIM structure can be further applied in the future to realize electrical control or electrical injection of plasmonic devices through graphene.

Surface-enhanced Raman spectroscopy (SERS) is an ultrasensitive technique to identify vibrational fingerprints of trace analytes. However, present SERS techniques suffer from the lack of uniform, reproducible, and stable substrates to control the plasmonic hotspots in a wide spectral range. Here, we report the promising application of epitaxial aluminum films as a scalable plasmonic platform for SERS applications. To assess the uniformity of aluminum substrates, atomically thin transition metal dichalcogenide monolayers are used as the benchmark analyte due to their inherent two-dimensional homogeneity. Besides the distinctive spectral capability of aluminum in the ultraviolet (325 nm), we demonstrate that the aluminum substrates can even perform comparably with the silver counterparts made from single-crystalline colloidal silver crystals using the same SERS substrate design in the visible range (532 nm). This is unexpected from the prediction solely based on optical dielectric functions and illustrate the superior surface and interface properties of epitaxial aluminum SERS substrates.