Methodology and implementation of a tunable deep-ultraviolet laser source for photoemission electron microscopy.

Photoemission electron microscopy (PEEM) is a unique and powerful tool for studying the electronic properties of materials and surfaces. However, it requires intense and well-controlled light sources with photon energies ranging from the UV to soft X-rays for achieving high spatial resolution and image contrast. Traditionally, many PEEMs were installed at synchrotron light sources to access intense and tunable soft X-rays. More recently, the maturation of solid-state lasers has opened a new avenue for laboratory-based PEEMs using laser-based UV light at lower photon energies. Here, we report on the characteristics of a laser-based UV light source that was recently integrated with a PEEM instrument. The system consists of a high repetition rate, tunable wavelength laser coupled to a harmonics generation module, which generates deep-UV radiation from 192 nm to 210 nm. We comment on the spectral characteristics and overall laser system stability, as well as on the effects of space charge within the PEEM microscope at high UV laser fluxes. Further, we show an example of imaging on gallium nitride, where the higher UV photon energy and flux of the laser provides considerably improved image quality, compared to a conventional light source. These results demonstrate the capabilities of laser-based UV light sources for advancing laboratory-based PEEMs.

Thermal conductivity measurements of sub-surface buried substrates by steady-state thermoreflectance.

Measuring the thermal conductivity of sub-surface buried substrates is of significant practical interests. However, this remains challenging with traditional pump-probe spectroscopies due to their limited thermal penetration depths. Here, we experimentally and numerically investigate the TPD of the recently developed optical pump-probe technique steady-state thermoreflectance (SSTR) and explore its capability for measuring the thermal properties of buried substrates. The conventional definition of the TPD (i.e., the depth at which temperature drops to 1/e value of the maximum surface temperature) does not truly represent the upper limit of how far beneath the surface SSTR can probe. For estimating the uncertainty of SSTR measurements of a buried substrate a priori, sensitivity calculations provide the best means. Thus, detailed sensitivity calculations are provided to guide future measurements. Due to the steady-state nature of SSTR, it can measure the thermal conductivity of buried substrates that are traditionally challenging by transient pump-probe techniques, exemplified by measuring three control samples. We also discuss the required criteria for SSTR to isolate the thermal properties of a buried film. Our study establishes SSTR as a suitable technique for thermal characterizations of sub-surface buried substrates in typical device geometries.

Development of solar-blind photodetectors based on Si-implanted ß-Ga(2)O(3).

ß-Ga(2)O(3) films grown on Al(2)O(3) by a metalorganic chemical vapor deposition technique were used to fabricate a solar-blind photodetector with a planar photoconductor structure. The crystal structure and quality of the ß-Ga(2)O(3) films were analyzed using X-ray diffraction and micro-Raman spectroscopy. Si ions were introduced into the ß-Ga(2)O(3) thin films by ion implantation method and activated by an annealing process to form an Ohmic contact between the Ti/Au electrode and the ß-Ga(2)O(3) film. The electrical conductivity of the ß-Ga(2)O(3) films was greatly improved by the implantation and subsequent activation of the Si ions. The photoresponse properties of the photodetectors were investigated by analyzing the current-voltage characteristics and the time-dependent photoresponse curves. The fabricated solar-blind photodetectors exhibited photoresponse to 254 nm wavelength, and blindness to 365 nm light, with a high spectral selectivity.

Electron backscatter diffraction study of hexagonal boron nitride growth on Cu single-crystal substrates.

Hexagonal boron nitride (h-BN) is an important material for the development of new 2D heterostructures. To enable this development, the relationship between crystal growth and the substrate orientation must be explored and understood. In this study, we simultaneously grew h-BN on different orientations of Cu substrates to establish the impact of substrate structure on the growth habit of thin h-BN layers. The substrates studied were a polycrystalline Cu foil, Cu(100), Cu(110), and Cu(111). Fourier transform grazing-incidence infrared reflection absorption spectroscopy (FT-IRRAS) was used to identify h-BN on copper substrates. X-ray photoelectron spectroscopy (XPS) was used to determine the effective thickness of the h-BN. Scanning electron microscopy (SEM) and electron backscatter diffraction (EBSD) were used to measure the morphology of the films and postgrowth crystal structure of the Cu substrates, respectively. Combining the SEM and EBSD images allowed for the correlation between h-BN film coverage and the crystal structure of Cu. It was found that the growth rate was inversely proportional to the surface free energy of the Cu surface, with Cu(111) having the most h-BN surface coverage. The Cu foil predominately crystallized with a (100) surface orientation, and likewise had a film coverage very close to the Cu(100).

Growth and spectroscopic characterization of monolayer and few-layer hexagonal boron nitride on metal substrates.

Atomically thin two dimensional hexagonal boron nitride (2D h-BN) is one of the key materials in the development of new van der Waals heterostructures due to its outstanding properties including an atomically smooth surface, high thermal conductivity, high mechanical strength, chemical inertness and high electrical resistance. The development of 2D h-BN growth is still in the early stages and largely depends on rapid and accurate characterization of the grown monolayer or few layers h-BN films. This paper demonstrates a new approach to characterizing monolayer h-BN films directly on metal substrates by grazing-incidence infrared reflection absorption spectroscopy (IRRAS). Using h-BN films grown by atmospheric-pressure chemical vapor deposition on Cu and Ni substrates, two new sub-bands are found for the A2u out-of-plane stretching mode. It is shown, using both experimental and computational methods, that the lower-energy sub-band is related to 2D h-BN coupled with substrate, while the higher energy sub-band is related to decoupled (or free-standing) 2D h-BN. It is further shown that this newly-observed fine structure in the A2u mode can be used to assess, quickly and easily, the homogeneity of the h-BN-metal interface and the effects of metal surface contamination on adhesion of the layer.

Chemical etching behaviors of semipolar (11̄22) and nonpolar (11̄20) gallium nitride films.

Wet chemical etching using hot KOH and H3PO4 solutions was performed on semipolar (11̄22) and nonpolar (11̄20) GaN films grown on sapphire substrates. An alternating KOH/H3PO4/KOH etch process was developed to control the orientation of the facets on the thin-film surface. The initial etch step in KOH produced c- and m-plane facets on the surface of both semipolar (11̄22) and nonpolar (11̄20) GaN thin-films. A second etch step in H3PO4 solution additionally exposed a (̄1̄12̄2) plane, which is chemically stable in H3PO4 solution. By repeating the chemical etch with KOH solution, the m-plane facets as seen in the original KOH etch step were recovered. The etching methods developed in our work can be used to control the surface morphologies of nonpolar and semipolar GaN-based optoelectronic devices such as light-emitting diodes and solar cells.

GaN-based ultraviolet light-emitting diodes with AuCl3-doped graphene electrodes.

We demonstrate AuCl3-doped graphene transparent conductive electrodes integrated in GaN-based ultraviolet (UV) light-emitting diodes (LEDs) with an emission peak of 363 nm. AuCl3 doping was accomplished by dipping the graphene electrodes in 5, 10 and 20 mM concentrations of AuCl3 solutions. The effects of AuCl3 doping on graphene electrodes were investigated by current-voltage characteristics, sheet resistance, scanning electron microscope, optical transmittance, micro-Raman scattering and electroluminescence images. The optical transmittance was decreased with increasing the AuCl3 concentrations. However, the forward currents of UV LEDs with p-doped (5, 10 and 20 mM of AuCl3 solutions) graphene transparent conductive electrodes at a forward bias of 8 V were increased by ~48, 63 and 73%, respectively, which can be attributed to the reduction of sheet resistance and the increase of work function of the graphene. The performance of UV LEDs was drastically improved by AuCl3 doping of graphene transparent conductive electrodes.

Single n-GaN microwire/p-Silicon thin film heterojunction light-emitting diode.

The emission and waveguiding properties of individual GaN microwires as well as devices based on an n-GaN microwire/p-Si (100) junction were studied for relevance in optoelectronics and optical circuits. Pulsed photoluminescence of the GaN microwire excited in the transverse or longitudinal direction demonstrated gain. These n-type GaN microwires were positioned mechanically or by dielectrophoretic force onto pre-patterned electrodes on a p-type Si (100) substrate. Electroluminescence from this p-n point junction was characteristic of a heterostructure light-emitting diode. Additionally, waveguiding was observed along the length of the microwire for light originating from photoluminescence as well as from electroluminescence generated at the p-n junction.

Epitaxial graphene nucleation on C-face silicon carbide.

The initial stages of epitaxial graphene growth were studied by characterization of graphene formed in localized areas on C-face 6H-SiC substrates. The graphene areas were determined to lie below the level of the surrounding substrate and showed different morphologies based on size. Employing electron channeling contrast imaging, the presence of threading screw dislocations was indicated near the centers of each of these areas. After the graphene was removed, these dislocations were revealed to lie within the SiC substrate. These observations suggest that screw dislocations act as preferred nucleation sites for graphene growth on C-face SiC.

Nanostructured n-ZnO / thin film p-silicon heterojunction light-emitting diodes.

Electroluminescence (EL) was obtained from a p-Si (100) thin film/nanostructured n-ZnO heterojunction diode fabricated by a simple dielectrophoresis (DEP) method. The Si substrate was pre-patterned with electrodes and an insulating separation layer by a standard photolithographic process. ZnO nanostructures were formed by a simple solution chemistry and subsequently transferred to the pre-patterned substrate. Application of the DEP force at a frequency of 100 kHz and 6 V peak-to-peak voltage allowed precise positioning of the ZnO nanostructures at the edge of the metal electrodes. The physically formed p-Si (100) thin film/nanostructured n-ZnO heterojunction displayed multi-color emission from the ZnO near band edge as well as emission from defective states within the ZnO band gap.

Quantum linear magnetoresistance in multilayer epitaxial graphene.

We report the first observation of linear magnetoresistance (LMR) in multilayer epitaxial graphene grown on SiC. We show that multilayer epitaxial graphene exhibits large LMR from 2.2 K up to room temperature and that it can be best explained by a purely quantum mechanical model. We attribute the observation of LMR to inhomogeneities in the epitaxially grown graphene film. The large magnitude of the LMR suggests potential for novel applications in areas such as high-density data storage and magnetic sensors and actuators.

Photopolymerization of self-assembled monolayers of diacetylenic alkylphosphonic acids on group-III nitride substrates.

This paper describes the fabrication and characterization of photopolymerizable alkylphosphonate self-assembled monolayers (SAMs) on group-III nitride substrates including GaN and Al(x)Ga(1-x)N (AlGaN; x = 0.2 and 0.25). Contact angle goniometry, visible absorption spectroscopy, and atomic force microscopy were used to assess the formation, desorption, and photopolymerization of SAMs of diacetylenic alkylphosphonic acids (CH(3)(CH(2))(n)-C[triple bond]C-C[triple bond]C-(CH(2))(m)PO(OH)(2); (m, n) = (3, 11), (6, 8), and (9, 5)). As with GaN substrates (Ito, T.; Forman, S. M.; Cao, C.; Li, F.; Eddy, C. R., Jr.; Mastro, M. A.; Holm, R. T.; Henry, R. L.; Hohn, K.; Edgar, J. H. Langmuir 2008, 24, 6630-6635), alkylphosphonic acids formed SAMs on UV/O(3)-treated AlGaN substrates from their toluene solutions in contrast to other primary substituted hydrocarbons with a terminal -COOH, -NH(2), -OH, or -SH group. Diacetylenic alkylphosphonate SAMs on group-III nitrides could be polymerized by UV irradiation (254 nm), as indicated by the appearance of a visible absorption band around 640 nm and also by their significantly reduced desorption from the surface in a 0.1 M aqueous NaOH solution. A longer UV irradiation time was required to maximize the photopolymerization of a SAM having a diacetylene group close to the terminal phosphonate moiety, probably because of the hindrance of the topochemical polymerization due to the limited flexibility of the cross-linking moieties on an atomically rough substrate surface.

Technique for the dry transfer of epitaxial graphene onto arbitrary substrates.

To make graphene technologically viable, the transfer of graphene films to substrates appropriate for specific applications is required. We demonstrate the dry transfer of epitaxial graphene (EG) from the C-face of 4H-SiC onto SiO(2), GaN and Al(2)O(3) substrates using a thermal release tape. Subsequent Hall effect measurements illustrated that minimal degradation in the carrier mobility was induced following the transfer process in lithographically patterned devices. Correspondingly, a large drop in the carrier concentration was observed following the transfer process, supporting the notion that a gradient in the carrier density is present in C-face EG, with lower values being observed in layers further removed from the SiC interface. X-ray photoemission spectra collected from EG films attached to the transfer tape revealed the presence of atomic Si within the EG layers, which may indicate the identity of the unknown intrinsic dopant in EG. Finally, this transfer process is shown to enable EG films amenable for use in device fabrication on arbitrary substrates and films that are deemed most beneficial to carrier transport, as flexible electronic devices or optically transparent contacts.