Applicability of the constitutive equations for the determination of the material properties of optically active materials.

For the description of the optical response of optically active media, different constitutive equations have been proposed and are still used in literature. Here, we demonstrate on potassium titanyl phosphate (KTiOPO4) by means of ellipsometry that only the symmetric constitutive equation describes the observed spectra properly and allows the unique determination of the gyration tensor.

Voigt Exceptional Points in an Anisotropic ZnO-Based Planar Microcavity: Square-Root Topology, Polarization Vortices, and Circularity.

Voigt points represent propagation directions in anisotropic crystals along which optical modes degenerate, leading to a single circularly polarized eigenmode. They are a particular class of exceptional points. Here, we report the fabrication and characterization of a dielectric, anisotropic optical microcavity based on nonpolar ZnO that implements a non-Hermitian system and mimics the behavior of Voigt points in natural crystals. We prove the exceptional-point nature by monitoring the complex-square-root topology of the mode eigenenergies (real and imaginary parts) around the Voigt points. Polarization state analysis shows that these artificially engineered Voigt points behave as vortex cores for the linear polarization and sustain chiral modes. Our findings apply to any planar microcavity with broken cylindrical symmetry and, thus, pave the way for exploiting exceptional points in widespread optoelectronic devices such as vertical cavity surface emitting lasers and resonant cavity light emitting diodes.

Room-temperature synthesized copper iodide thin film as degenerate p-type transparent conductor with a boosted figure of merit.

A degenerate p-type conduction of cuprous iodide (CuI) thin films is achieved at the iodine-rich growth condition, allowing for the record high room-temperature conductivity of ∼156 S/cm for as-deposited CuI and ∼283 S/cm for I-doped CuI. At the same time, the films appear clear and exhibit a high transmission of 60-85% in the visible spectral range. The realization of such simultaneously high conductivity and transparency boosts the figure of merit of a p-type TC: its value jumps from ∼200 to ∼17,000 MΩ-1 Polycrystalline CuI thin films were deposited at room temperature by reactive sputtering. Their electrical and optical properties are examined relative to other p-type transparent conductors. The transport properties of CuI thin films were investigated by temperature-dependent conductivity measurements, which reveal a semiconductor-metal transition depending on the iodine/argon ratio in the sputtering gas.

Spatiotemporal Evolution of Coherent Polariton Modes in ZnO Microwire Cavities at Room Temperature.

Tunable waveguides for propagating coherent quantum states are demanded for future applications in quantum information technology and optical data processing. We present coherent whispering gallery mode polariton states in ZnO-based hexagonal microwires at room temperature. We observed their propagation over the field of view of about 20 µm by picosecond time-resolved real space imaging using a streak camera. Spatial coherence was proven by time integrated Michelson interferometry superimposing the inverted spatial emission pattern with its original one. We furthermore show that the real and momentum space evolution of the coherent states can not only be described by the commonly used model developed for ballistically propagating Bose-Einstein condensates based on the Gross-Pitaevskii equation but equivalently by classical ray optics considering a spatially varying particle density dependent refractive index of the cavity material, not yet considered in literature so far. By changing the excitation spot size, the refractive index gradient and thus the propagation velocity is changed.

Defect Manipulation To Control ZnO Micro-/Nanowire-Metal Contacts.

Surface states that induce depletion regions are commonly believed to control the transport of charged carriers through semiconductor nanowires. However, direct, localized optical, and electrical measurements of ZnO nanowires show that native point defects inside the nanowire bulk and created at metal-semiconductor interfaces are electrically active and play a dominant role electronically, altering the semiconductor doping, the carrier density along the wire length, and the injection of charge into the wire. We used depth-resolved cathodoluminescence spectroscopy to measure the densities of multiple point defects inside ZnO nanowires, substitutional Cu on Zn sites, zinc vacancy, and oxygen vacancy defects, showing that their densities varied strongly both radially and lengthwise for tapered wires. These defect profiles and their variation with wire diameter produce trap-assisted tunneling and acceptor trapping of free carriers, the balance of which determines the low contact resistivity (2.6 × 10-3 Ω·cm-2) ohmic, Schottky (Φ ≥ 0.35 eV) or blocking nature of Pt contacts to a single nano/microwire. We show how these defects can now be manipulated by ion beam methods and nanowire design, opening new avenues to control nanowire charge injection and transport.

Dynamical Tuning of Nanowire Lasing Spectra.

Realizing visionary concepts of integrated photonic circuits, nanospectroscopy, and nanosensing will tremendously benefit from dynamically tunable coherent light sources with lateral dimensions on the subwavelength scale. Therefore, we demonstrate an individual nanowire laser based device which can be gradually tuned by reversible length changes of the nanowire such that uniaxial tensile stress is applied to the respective semiconductor gain material. By straining the device, the spontaneous excitonic emission of the nanowire shifts to lower energies caused by the bandgap reduction of the semiconductor. Moreover, the optical gain spectrum of the nanolaser can be precisely strain-tuned in the high excitation regime. The tuning of the emission does not affect the laser threshold of the device, which is very beneficial for practical applications. The applied length change furthermore adjusts the laser resonances inducing a redshift of the longitudinal modes. Thus, this concept of gradually and dynamically tunable nanolasers enables controlling and modulating the coherent emission on the nanoscale without changing macroscopic ambient conditions. This concept holds therefore huge impact on nanophotonic switches and photonic circuit technology.

Raman Tensor Formalism for Optically Anisotropic Crystals.

We present a formalism for calculating the Raman scattering intensity dependent on the polarization configuration for optically anisotropic crystals. It can be applied to crystals of arbitrary orientation and crystal symmetry measured in normal incidence backscattering geometry. The classical Raman tensor formalism cannot be used for optically anisotropic materials due to birefringence causing the polarization within the crystal to be depth dependent. We show that in the limit of averaging over a sufficiently large scattering depth, the observed Raman intensities converge and can be described by an effective Raman tensor given here. Full agreement with experimental results for uniaxial and biaxial crystals is demonstrated.

Carrier density driven lasing dynamics in ZnO nanowires.

We report on the temporal lasing dynamics of high quality ZnO nanowires using the time-resolved micro-photoluminescence technique. The temperature dependence of the lasing characteristics and of the corresponding decay constants demonstrate the formation of an electron-hole plasma to be the underlying gain mechanism in the considered temperature range from 10 K to 300 K. We found that the temperature-dependent emission onset-time ([Formula: see text]) strongly depends on the excitation power and becomes smallest in the lasing regime, with values below 5 ps. Furthermore, the observed red shift of the dominating lasing modes in time is qualitatively discussed in terms of the carrier density induced change of the refractive index dispersion after the excitation laser pulse. This theory is supported by extending an existing model for the calculation of the carrier density dependent complex refractive index for different temperatures. This model coincides with the experimental observations and reliably describes the evolution of the refractive index after the excitation laser pulse.

Conducting behavior of chalcopyrite-type CuGaS2 crystals under visible light.

Millimeter size high quality crystals of CuGaS2 were grown by chemical vapor transport. The highly ordered chalcopyrite structure is confirmed by X-ray diffraction and Raman spectroscopy. According to energy dispersive X-ray spectroscopy the composition of the crystals is very close to the formula CuGaS2. Room temperature photoluminescence measurements indicate the presence of an emission peak at about 2.36 eV that can be related to a donor-acceptor pair transition. The electrical resistance as a function of temperature is very well described by the Mott variable range hopping mechanism. Room temperature complex impedance spectroscopy measurements were performed in the alternating current frequency range from 40 to 10(7) Hz in the dark and under normal light. According to the impedance spectroscopy data the experimental results can be well described by two circuits in series, corresponding to bulk and grain boundary contributions. An unusual positive photoresistance effect is observed in the frequency range between 3 and 30 kHz, which we suggest to be due to intrinsic defects present in the CuGaS2 crystal.

Flexible hardware concept of pulsed laser deposition for large areas and combinatorial composition spreads.

Pulsed laser deposition (PLD) is one of the most flexible physical growth techniques for thin films of functional materials at the research and demonstrator level. We describe here a relatively simple and reliable concept of the PLD hardware that allows both deposition on large areas up to 4 in. diameter and deposition of tailored lateral and vertical composition spreads without time-consuming hardware changes. Different PLD approaches have been implemented in various chambers via specific and correlated computer-controlled movements of the target, substrate, and masks in conjunction with an appropriate target phase composition. The design of the chambers benefits from our long-term experience to find the most reliable solutions for the critical mechanical and high-temperature parts.

Growth of κ-([Al,In]xGa1-x)2O3 Quantum Wells and Their Potential for Quantum-Well Infrared Photodetectors.

The wide band gap semiconductor κ-Ga2O3 and its aluminum and indium alloys have been proposed as promising materials for many applications. One of them is the use of inter-sub-band transitions in quantum-well (QW) systems for infrared detectors. Our simulations show that the detection wavelength range of nowadays state of the art GaAs/AlxGa1-xAs quantum-well infrared photodetectors (QWIPs) could be substantially excelled with about 1-100 µm using κ-([Al,In]xGa1-x)2O3, while at the same time being transparent to visible light and therefore insensitive to photon noise due to its wide band gap, demonstrating the application potential of this material system. Our simulations further show that the QWIPs efficiency critically depends on the QW thickness, making a precise control over the thickness during growth and a reliable thickness determination essential. We demonstrate that pulsed laser deposition yields the needed accuracy, by analyzing a series of (InxGa1-x)2O3 QWs with (AlyGa1-y)2O3 barriers with high-resolution X-ray diffraction, X-ray photoelectron spectroscopy (XPS) depth profiling, and transmission electron microscopy (TEM). While the superlattice fringes of high-resolution X-ray diffraction only yield an average combined thickness of the QWs and the barrier and X-ray spectroscopy depth profiling requires elaborated modeling of the XPS signal to accurately determine the thickness of such QWs, TEM is the method of choice when it comes to the determination of QW thicknesses.

Amorphous Transparent Cu(S,I) Thin Films with Very High Hole Conductivity.

Amorphous transparent conductors (a-TCs) are key materials for flexible and transparent electronics but still suffer from poor p-type conductivity. By developing an amorphous Cu(S,I) material system, record high hole conductivities of 103-104 S cm-1 have been achieved in p-type a-TCs. These high conductivities are comparable with commercial n-type TCs made of indium tin oxide and are 100 times greater than any previously reported p-type a-TCs. Responsible for the high hole conduction is the overlap of large p-orbitals of I- and S2- anions, which provide a hole transport pathway insensitive to structural disorder. In addition, the bandgap of amorphous Cu(S,I) can be modulated from 2.6 to 2.9 eV by increasing the iodine content. These unique properties demonstrate that the Cu(S,I) system holds great potential as a promising p-type amorphous transparent electrode material for optoelectronics.

Suppression of Rotational Domains of CuI Employing Sodium Halide Buffer Layers.

The occurrence of rotational domains is a well-known issue for copper iodide (CuI) that naturally occurs for growth on popular substrates like sapphire. However, this has detrimental effects on the thin film quality like increasing surface roughness or deteriorated transport characteristics due to grain boundary scattering. Utilizing pulsed laser deposition and the in situ growth of sodium chloride (NaCl) and sodium bromide (NaBr) template layers, studies were performed on their potential on suppressing the formation of rotational domains of CuI on c-plane sapphire and SrF2(111) substrates. Corresponding samples were investigated concerning their epitaxial properties and further characterized regarding (volume) crystalline, morphological, and electrical properties. Particularly for NaBr template layers, fully single-crystalline growth of CuI thin films was obtained and resulted in significantly reduced surface roughness of the CuI layer.

Mid- and far-infrared localized surface plasmon resonances in chalcogen-hyperdoped silicon.

Plasmonic sensing in the infrared region employs the direct interaction of the vibrational fingerprints of molecules with the plasmonic resonances, creating surface-enhanced sensing platforms that are superior to traditional spectroscopy. However, the standard noble metals used for plasmonic resonances suffer from high radiative losses as well as fabrication challenges, such as tuning the spectral resonance positions into mid- to far-infrared regions, and the compatibility issue with the existing complementary metal-oxide-semiconductor (CMOS) manufacturing platform. Here, we demonstrate the occurrence of mid-infrared localized surface plasmon resonances (LSPR) in thin Si films hyperdoped with the known deep-level impurity tellurium. We show that the mid-infrared LSPR can be further enhanced and spectrally extended to the far-infrared range by fabricating two-dimensional arrays of micrometer-sized antennas in a Te-hyperdoped Si chip. Since Te-hyperdoped Si can also work as an infrared photodetector, we believe that our results will unlock the route toward the direct integration of plasmonic sensors with the on-chip CMOS platform, greatly advancing the possibility of mass manufacturing of high-performance plasmonic sensing systems.

Indium Gallium Oxide Alloys: Electronic Structure, Optical Gap, Surface Space Charge, and Chemical Trends within Common-Cation Semiconductors.

The electronic and optical properties of (InxGa1-x)2O3 alloys are highly tunable, giving rise to a myriad of applications including transparent conductors, transparent electronics, and solar-blind ultraviolet photodetectors. Here, we investigate these properties for a high quality pulsed laser deposited film which possesses a lateral cation composition gradient (0.01 ≤ x ≤ 0.82) and three crystallographic phases (monoclinic, hexagonal, and bixbyite). The optical gaps over this composition range are determined, and only a weak optical gap bowing is found (b = 0.36 eV). The valence band edge evolution along with the change in the fundamental band gap over the composition gradient enables the surface space-charge properties to be probed. This is an important property when considering metal contact formation and heterojunctions for devices. A transition from surface electron accumulation to depletion occurs at x ∼ 0.35 as the film goes from the bixbyite In2O3 phase to the monoclinic ß-Ga2O3 phase. The electronic structure of the different phases is investigated by using density functional theory calculations and compared to the valence band X-ray photoemission spectra. Finally, the properties of these alloys, such as the n-type dopability of In2O3 and use of Ga2O3 as a solar-blind UV detector, are understood with respect to other common-cation compound semiconductors in terms of simple chemical trends of the band edge positions and the hydrostatic volume deformation potential.

Occurrence of rotation domains in heteroepitaxy.

Heteroepitaxy can involve materials with a misfit of crystal structure. Rotation domains in the epilayer are a fundamental consequence. We derive a general expression for their (minimum) number which is determined by the mismatch of the rotational symmetries of the substrate and epilayer. In the case of a mismatch of rotational symmetry, the number of rotation domains of material A on material B is different from that of B on A. A larger number of rotation domains can occur due to domain structure or nearly fulfilled additional symmetries of the substrate surface.

Gold nanostructure matrices by diffraction mask-projection laser ablation: extension to previously inaccessible substrates.

Gold nanodot matrices made by diffraction mask-projection laser ablation (DiMPLA) are presented. The nanodots are well ordered and can be synthesized on so far not accessible substrates by virtue of intermediate thin AlO(x) layers deposited by pulsed-laser deposition (PLD). Investigations were made on the influence of layer thickness, roughness and type of substrate on the nanodots and their fabrication. It is shown that all of these parameters are crucial for the generation of nanodots on thin AlO(x) layers. The roughness of the layer and the substrate material determine whether the layer cracks upon laser patterning. The layer thickness, on the other hand, influences the size of gold nanodots on top. Extinction spectra show that the particle size is the dominant contribution that shifts the plasmon resonance peak.

The principal axes systems for the elastic properties of monoclinic gallia.

We discuss the principal axes systems of monoclinic and triclinic crystals regarding their elastic properties. Explicit formulas are presented for the orientation of these coordinate systems for monoclinic crystals. In this context, theoretical results from literature on the elastic properties of monoclinic (space group C2/m) gallia and alumina are critically discussed.

Band Offsets at κ-([Al,In]xGa1-x)2O3/MgO Interfaces.

Conduction and valence band offsets are among the most crucial material parameters for semiconductor heterostructure device design, such as for high-electron mobility transistors or quantum well infrared photodetectors (QWIP). Because of its expected high spontaneous electrical polarization and the possibility of polarization doping at heterointerfaces similar to the AlGaN/InGaN/GaN system, the metastable orthorhombic κ-phase of Ga2O3 and its indium and aluminum alloy systems are a promising alternative for such device applications. However, respective band offsets to any dielectric are unknown, as well as the evolution of the bands within the alloy systems. We report on the valence and conduction band offsets of orthorhombic κ-(AlxGa1-x)2O3 and κ-(InxGa1-x)2O3 thin films to MgO as reference dielectric by X-ray photoelectron spectroscopy. The thin films with compositions xIn ≤ 0.27 and xAl ≤ 0.55 were grown by pulsed laser deposition utilizing tin-doped and radially segmented targets. The determined band alignments reveal the formation of a type I heterojunction to MgO for all compositions with conduction band offsets of at least 1.4 eV, providing excellent electron confinement. Only low valence band offsets with a maximum of ∼300 meV were observed. Nevertheless, this renders MgO as a promising gate dielectric for metal-oxide-semiconductor transistors in the orthorhombic modification. We further found that the conduction band offsets in the alloy systems are mainly determined by the evolution of the band gaps, which can be tuned by the composition in a wide range between 4.1 and 6.2 eV, because the energy position of the valence band maximum remains almost constant over the complete composition range investigated. Therefore, tunable conduction band offsets of up to 1.1 eV within the alloy systems allow for subniveau transition energies in (AlxGa1-x)2O3/(InxGa1-x)2O3/(AlxGa1-x)2O3 quantum wells from the infrared to the visible regime, which are promising for application in QWIPs.

Enhanced Magnetoelectric Coupling in BaTiO3-BiFeO3 Multilayers-An Interface Effect.

Combining various (multi-)ferroic materials into heterostructures is a promising route to enhance their inherent properties, such as the magnetoelectric coupling in BiFeO3 thin films. We have previously reported on the up-to-tenfold increase of the magnetoelectric voltage coefficient α ME in BaTiO3-BiFeO3 multilayers relative to BiFeO3 single layers. Unraveling the origin and mechanism of this enhanced effect is a prerequisite to designing new materials for the application of magnetoelectric devices. By careful variations in the multilayer design we now present an evaluation of the influences of the BaTiO3-BiFeO3 thickness ratio, oxygen pressure during deposition, and double layer thickness. Our findings suggest an interface driven effect at the core of the magnetoelectric coupling effect in our multilayers superimposed on the inherent magnetoelectric coupling of BiFeO3 thin films, which leads to a giant α ME coefficient of 480 V c m -1 Oe-1 for a 16 × (BaTiO3-BiFeO3) superlattice with a 4 . 8 nm double layer periodicity.